Anisotropic growth of ZnO nanorod arrays on ZnO thin films was achieved at a temperature of 90° C by a surfactant-assisted soft chemical approach with control over size and orientation. ZnO thin films with c-axis preferred orientation had been achieved by the sol-gel technique. Lengths, diameters, and the degree of alignment of the ZnO nanorods were controlled by changing the experimental parameters. It was observed that the surfactant was essential to restrict the lateral growth of the nanorods, whereas the pH level of the reaction medium controlled the length of the nanorods. On the other hand, the orientation of the nanorods depended on the crystalline orientation of the film as well as the pH of the reaction medium. Room-temperature photoluminescence studies revealed that the ZnO nanorods with the best alignment exhibited the best emission property. The ZnO nanorods exhibited a strong UV emission peak at ∼3.22 eV, ascribed to the band-edge emission. The field emission studies of the well-aligned nanorod arrays exhibited a low turn-on field of 1.7 V/μm to get an emission current density of 0.1 μA/cm2.